M. V. Okhapkin

We present measurements on a metastable state in $\mathrm{Th}^{2+}$ with the electronic configuration $6d^2\,{}^3P_0\,(5090\ \mathrm{cm^{-1}})$. This is motivated by the prospect of using the state in laser excitation of the low-energy $^{229}$Th nuclear resonance independent from the leading hyperfine interactions. The $6d^2\,{}^3P_0$ state has no dipole-allowed radiative decay channel and is connected to the second ground state $6d^2\,{}^3F_2\,(63\ \mathrm{cm^{-1}})$ through an electric quadrupole transition only. We populate the state by laser excitation at 484~nm via a higher excited level and detect its population in laser-induced fluorescence. The isotope shift of the $J=0$ level between $^{232}\mathrm{Th}^{2+}$ and $^{229}\mathrm{Th}^{2+}$ is determined as a measure of the interaction of electronic and nuclear charge distributions. The lifetime of the level in our ion trap with buffer gas is limited by collisional mixing with the nearby state $5f6d\,{}^3G_3\,(5060\ \mathrm{cm^{-1}})$. In ultrahigh vacuum, it could serve as a hyperfine-free nuclear clock that is largely immune to field-induced frequency shifts via the electron shell.

The hyperfine structure of $^{229}$Th$^{3+}$ ions in the nuclear ground state is investigated via laser spectroscopy of trapped Th$^{3+}$ ions that are sympathetically cooled by laser-cooled $^{88}$Sr$^+$ ions in a linear Paul trap. The isotope shift to $^{230}$Th$^{3+}$ and the hyperfine constants for the magnetic dipole (A) and electric quadrupole (B) interactions for the 5F$_{5/2}$ and 6D$_{5/2}$ electronic states of $^{229}$Th$^{3+}$ are determined. These measurements provide nuclear moments of $^{229}$Th with reduced uncertainty and serve as a preparation for improved hyperfine spectroscopy of the 8.4 eV nuclear isomeric state in $^{229}$Th$^{3+}$ ions.

Sympathetic cooling of Th$^{3+}$ ions is demonstrated in an experiment where $^{229}$Th and $^{230}$Th are extracted from uranium recoil ion sources and are confined in a linear Paul trap together with laser-cooled $^{88}$Sr$^+$ ions. Because of their similar charge-to-mass ratios the ions are closely coupled and arrange themselves in two-species Coulomb crystals, containing up to a few tens of Th$^{3+}$ ions. To show the suitability of the sympathetically cooled Th$^{3+}$ ions for high-resolution laser spectroscopy, the absolute frequencies and isotope shifts of 5F$_{5/2}$\,$\rightarrow$\,6D$_{5/2}$ and 5F$_{7/2}$\,$\rightarrow$\,6D$_{5/2}$ transitions of $^{230}$Th$^{3+}$ have been measured. The system is developed for hyperfine spectroscopy of electronic transitions of nuclear ground and isomeric states in $^{229}$Th$^{3+}$.

Using resonant two-step laser excitation of trapped 232Th+ ions, we observe 43 previously unknown energy levels within the energy range from 7.3 to 8.3 eV. The high density of states promises a strongly enhanced electronic bridge excitation of the 229mTh nuclear state that is expected in this energy range. From the observation of resonantly enhanced three-photon ionization of Th+, the second ionization potential of thorium can be inferred to lie within the range between 11.9 and 12.3 eV. Pulsed laser radiation in a wide wavelength range from 237 to 289 nm is found to provide efficient photodissociation of molecular ions that are formed in reactions of Th+ with impurities in the buffer gas, leading to a significantly increased storage time for Th+ in the ion trap.

Experiments on one- and two-photon laser excitation of 232Th+ ions in a radiofrequency ion trap are reported. As the first excitation step, the strongest resonance line at 402 nm from the 6d^2 7s J=3/2 ground state to the 6d7s7p J=5/2 state at 24874 cm^{-1} is driven by radiation from an extended cavity diode laser. Spontaneous decay of the intermediate state populates a number of low-lying metastable states, thus limiting the excited state population and fluorescence signal obtainable with continuous laser excitation. We study the collisional quenching efficiency of helium, argon, and nitrogen buffer gases, and the effect of repumping laser excitation from the three lowest-lying metastable levels. The experimental results are compared with a four-level rate equation model, that allows us to deduce quenching rates for these buffer gases. Using laser radiation at 399 nm for the second step, we demonstrate two-photon excitation to the state at 49960 cm^{-1}, among the highest-lying classified levels of Th+. This is of interest as a test case for the search for higher-lying levels in the range above 55000 cm^{-1} which can resonantly enhance the excitation of the 229Th+ nuclear resonance through an inverse two-photon electronic bridge process.

The production of ions via laser ablation for the loading of radiofrequency (RF) ion traps is investigated using a nitrogen laser with a maximum pulse energy of 0.17 mJ and a peak intensity of about 250 MW/cm^2. A time-of-flight mass spectrometer is used to measure the ion yield and the distribution of the charge states. Singly charged ions of elements that are presently considered for the use in optical clocks or quantum logic applications could be produced from metallic samples at a rate of the order of magnitude 10^5 ions per pulse. A linear Paul trap was loaded with Th+ ions produced by laser ablation. An overall ion production and trapping efficiency of 10^-7 to 10^-6 was attained. For ions injected individually, a dependence of the capture probability on the phase of the RF field has been predicted. In the experiment this was not observed, presumably because of collective effects within the ablation plume.